Binder-free graphene oxide doughs.

Graphene oxide (GO) sheets have been used to construct various bulk forms of GO and graphene-based materials through solution-based processing techniques. Here, we report a highly cohesive dough state of GO with tens of weight percent loading in water without binder-like additives. The dough state can be diluted to obtain gels or dispersions, and dried to yield hard solids. It can be kneaded without leaving stains, readily reshaped, connected, and further processed to make bulk GO and graphene materials of arbitrary form factors and tunable microstructures. The doughs can be transformed to dense glassy solids of GO or graphene without long-range stacking order of the sheets, which exhibit isotropic and much enhanced mechanical properties due to hindered sliding between the sheets. GO dough is also found to be a good support material for electrocatalysts as it helps to form compliant interface to access the active particles.

A Cut-and-Paste Approach to 3D Graphene-Oxide-Based Architectures.

Properly cut sheets can be converted into complex 3D structures by three basic operations including folding, bending, and pasting to render new functions. Folding and bending are extensively employed in crumpling, origami, and pop-up fabrications for 3D structures. Pasting joins different parts of a material together, and can create new geometries that are fundamentally unattainable by folding and bending. However, it has been much less explored, likely due to limited choice of weldable thin film materials and residue-free glues. Here it is shown that graphene oxide (GO) paper is one such suitable material. Stacked GO sheets can be readily loosened up and even redispersed in water, which upon drying, restack to form solid structures. Therefore, water can be utilized to heal local damage, glue separated pieces, and release internal stress in bent GO papers to fix their shapes. Complex and dynamic 3D GO architectures can thus be fabricated by a cut-and-paste approach, which is also applicable to GO-based hybrid with carbon nanotubes or clay sheets.

Hot-pressed polymer nanofiber supported graphene membrane for high-performance nanofiltration.

Graphene oxide (GO) sheets can be readily surface-overlaid on hot-pressed electrospun polyacrylonitrile (PAN) nanofiber membrane to form a continuous and crack-free layer; upon thermal reduction at 150 °C for 12 h, the resulting reduced GO (rGO) layer can reject ∼90% MgSO4 with high water flux (due to the size exclusion mechanism), making the prepared PAN-rGO membranes promising nanofiltration media for water purification. It is important to note that no delamination of GO/rGO sheet layers has been observed throughout this study. We highlight that a simple processing method (i.e., hot pressing) is critical for the successful preparation of 2D materials (e.g., GO/rGO) based membranes/media. It is envisioned that the reported study can benefit many groups working on various membrane applications of 2D materials; in other words, the hot-pressed electrospun nanofiber membranes could be generally utilized as an innovative type of platform to support various 2D sheets for different separation applications such as highly efficient and cost-effective removal of dissolved components (e.g., organic molecules) and even (hydrated) ions from water.

On the origin of the stability of graphene oxide membranes in water.

Graphene oxide (GO) films are known to be highly stable in water and this property has made their use in membrane applications in solution possible. However, this state of affairs is somewhat counterintuitive because GO sheets become negatively charged on hydration and the membrane should disintegrate owing to electrostatic repulsion. We have now discovered a long-overlooked reason behind this apparent contradiction. Our findings show that neat GO membranes do, indeed, readily disintegrate in water, but the films become stable if they are crosslinked by multivalent cationic metal contaminants. Such metal contaminants can be introduced unintentionally during the synthesis and processing of GO, most notably on filtration with anodized aluminium oxide filter discs that corrode to release significant amounts of aluminium ions. This finding has wide implications in interpreting the processing-structure-property relationships of GO and other lamellar membranes. We also discuss strategies to avoid and mitigate metal contamination and demonstrate that this effect can be exploited to synthesize new membrane materials.